CN105380909A - Florfenicol soluble powder and preparation method thereof - Google Patents
Florfenicol soluble powder and preparation method thereof Download PDFInfo
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- CN105380909A CN105380909A CN201510996047.2A CN201510996047A CN105380909A CN 105380909 A CN105380909 A CN 105380909A CN 201510996047 A CN201510996047 A CN 201510996047A CN 105380909 A CN105380909 A CN 105380909A
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K9/00—Medicinal preparations characterised by special physical form
- A61K9/14—Particulate form, e.g. powders, Processes for size reducing of pure drugs or the resulting products, Pure drug nanoparticles
- A61K9/141—Intimate drug-carrier mixtures characterised by the carrier, e.g. ordered mixtures, adsorbates, solid solutions, eutectica, co-dried, co-solubilised, co-kneaded, co-milled, co-ground products, co-precipitates, co-evaporates, co-extrudates, co-melts; Drug nanoparticles with adsorbed surface modifiers
- A61K9/146—Intimate drug-carrier mixtures characterised by the carrier, e.g. ordered mixtures, adsorbates, solid solutions, eutectica, co-dried, co-solubilised, co-kneaded, co-milled, co-ground products, co-precipitates, co-evaporates, co-extrudates, co-melts; Drug nanoparticles with adsorbed surface modifiers with organic macromolecular compounds
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K31/00—Medicinal preparations containing organic active ingredients
- A61K31/16—Amides, e.g. hydroxamic acids
- A61K31/165—Amides, e.g. hydroxamic acids having aromatic rings, e.g. colchicine, atenolol, progabide
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K9/00—Medicinal preparations characterised by special physical form
- A61K9/0087—Galenical forms not covered by A61K9/02 - A61K9/7023
- A61K9/0095—Drinks; Beverages; Syrups; Compositions for reconstitution thereof, e.g. powders or tablets to be dispersed in a glass of water; Veterinary drenches
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Abstract
The invention discloses florfenicol soluble powder and a preparation method thereof. The soluble powder is composed of a florfenicol polydopamine compound and a substrate diluent. A preparation method of the florfenicol polydopamine compound comprises the following steps that 1, a surface active agent and florfenicol are added to an alkalescent solution and evenly mixed to obtain a mixture A, wherein the surface active agent can be added or not added; 2, dopamine hydrochloride is added to the mixture A, stirring is continuously conducted, a mixture B is obtained, spray drying is conducted, and the florfenicol polydopamine compound is obtained. The preparation method of the florfenicol soluble powder comprises the steps that 1, the substrate diluent and the florfenicol polydopamine compound are weighed through calculation, then the florfenicol polydopamine compound and the substrate diluent are mixed to be uniform, and the florfenicol soluble powder is obtained. The florfenicol soluble powder contains the florfenicol polydopamine compound, solubility of the florfenicol can be effectively improved, and the dissolving-out speed can be increased. The method is simple and easy to carry out, the time needed in preparation is short, and the production energy consumption is small.
Description
Technical field
The present invention relates to veterinary antibiotic preparation technique field, be specifically related to a kind of florfenicol soluble powder and preparation method thereof.
Background technology
Florfenicol is chloromycetin veterinary special broad-spectrum antibiotic of new generation, there is the features such as has a broad antifungal spectrum, good absorbing, distribution in vivo are wide, highly effective and safe, remarkable for the bacterial disease of fowl therapeutic effect caused by sensitive organism, have effect to gram positive bacteria and negative bacterium, be Bacillus typhi, the drug of first choice of various infection that Salmonella paratyphi, Salmonella cause.Because chloromycetin has the untoward reaction of serious induced aplastic anemia, forbidden for food animal, therefore, on animal diseases control, especially food animal, florfenicol has broad application prospects.But because florfenicol solubility is low, for non-water-soluble powder, absorption in animal body and bioavailability low, administration is carried out often by being mixed in feedstuff during administration, limit giving full play to of drug effect, and when there is more serious infection, often due to animal feed intake degradation, even appetite is absolutely useless, poor by mixed feeding drug treatment effect.But now the amount of drinking water of animal is normal, drinking water administration can ensure curative effect, and therefore exploitation is applicable to the drinking agent of poultry administration, will greatly improve the effect of florfenicol in poultry treating bacteriosis.The technology of current China florfenicol water soluble is primarily of flux method, solid dispersion method, ultra micro etc., but the solubilization-aid effect of these methods is undesirable, and dissolution velocity is slow, and dissolution is little, is difficult to meet preparation and dense demand of joining use.
Summary of the invention
For solving above-mentioned prior art Problems existing, the invention provides a kind of florfenicol soluble powder, dopamine complex is gathered containing florfenicol in this soluble powder, it is be coated in by florfenicol in the poly-dopamine of dopamine auto polymerization formation that florfenicol gathers dopamine complex, this complex effectively can improve dissolubility, the dissolution rate of florfenicol, is convenient to drinking water administration.
The present invention also provides a kind of preparation method of florfenicol soluble powder, and the method is simple, and the time needed for preparation is short, and energy consumption is little, is conducive to large-scale production and popularization.
Realizing the technical scheme that above-mentioned purpose of the present invention adopts is:
A kind of florfenicol soluble powder, gathers dopamine complex by florfenicol and matrix diluent forms:
The preparation method that described florfenicol gathers dopamine complex is as follows:
1) florfenicol powder is added in weak caustic solution, stirring and evenly mixing under room temperature, obtains mixture A; Or surfactant and florfenicol powder are added in weak caustic solution, stirring and evenly mixing under room temperature, obtain mixture A;
2) dopamine hydrochloride powder is joined in mixture A, wherein the mass ratio of florfenicol, dopamine hydrochloride, surfactant and weak caustic solution is 20:0.5-1:0-5:250, continue to stir 0.5-2 hour, obtain mixture B, mixture B is carried out spraying dry, obtains pulverous florfenicol and gather dopamine complex.
Described weak caustic solution is the sodium hydroxide solution of pH=8.5.
Described matrix diluent is any one in maltodextrin, dextrose plus saccharose, or 2-3 kind arbitrarily.
Described matrix diluent is glucose.
Described surfactant is PLURONICS F87 or Tween 80.
In described florfenicol soluble powder, the content of florfenicol is 10wt% or 20wt%.
Step 2) in, spraying dry inlet temperature is 160 DEG C-180 DEG C, leaving air temp 80 DEG C-90 DEG C, peristaltic pump rotating speed 140rpm.
A preparation method for florfenicol soluble powder, comprises the steps:
1) first measure florfenicol and gather the drug loading of dopamine complex, then calculated by the content of the florfenicol in this drug loading and required florfenicol soluble powder need to add matrix diluent, amount that florfenicol gathers dopamine complex;
2) florfenicol is gathered dopamine complex and matrix diluent is placed in mixer, stirring and evenly mixing, i.e. this florfenicol soluble powder obtained.
In obtained florfenicol soluble powder, the content of florfenicol is 10wt% or 20wt%.
Compared with prior art, its beneficial effect and advantage are in the present invention:
1) the present invention will gather dopamine and florfenicol compound first, obtain florfenicol by spray drying method again and gather dopamine complex, florfenicol gathers dissolubility, the dissolution rate that dopamine complex not only effectively can improve florfenicol, be convenient to drinking water administration, drug releasing rate can also be delayed, the action time of prolong drug, thus play long-acting, slow releasing function.Auto polymerization reaction condition due to dopamine is room temperature, and the response time is short, and therefore the preparation technology of this complex is simple, and energy consumption is low, and the time is short, is applicable to large-scale production and popularization.
2) the florfenicol soluble powder good water solubility obtained by the present invention, the dissolubility of florfenicol can bring up to 3000ppm, can meet the dense requirement of joining drinking water administration of poultry.
3) florfenicol soluble powder preparation method of the present invention and existing florfenicol soluble powder preparation method compared to, technique is comparatively easy, and operability is stronger, and energy consumption is less, and production cost is lower, is more conducive to large-scale production and popularization.
Detailed description of the invention
Below in conjunction with specific embodiment, the present invention is described in detail.
Embodiment 1
A kind of florfenicol soluble powder, its preparation method is as follows:
1) join in the sodium hydroxide solution of 250gpH=8.5 by 20g florfenicol powder stock medicine and 5g PLURONICS F87, stir 15min, mix homogeneously, obtains mixture A.
2) 1g dopamine hydrochloride is joined in mixture A, continue stirring 1 hour, obtain mixture B, mixture B is carried out spraying dry, controlling inlet temperature is 170 DEG C, leaving air temp 85 DEG C, peristaltic pump rotating speed 140rpm, obtains Powdered florfenicol and gathers dopamine complex, after testing, the drug loading that florfenicol gathers dopamine complex is 65.4%, and envelop rate is 95.2%.
3) content of the florfenicol gathered in the drug loading of dopamine complex and obtained florfenicol soluble powder according to florfenicol calculates the weight ratio that glucose and florfenicol gather dopamine complex.
4) weight ratio of gathering dopamine complex according to the glucose that calculates and florfenicol takes glucose and florfenicol gathers dopamine complex, again florfenicol is gathered dopamine complex and glucose is placed in mixer, stir 15min, mix homogeneously, namely obtained florfenicol weight percentage is the florfenicol soluble powder of 10% or 20%, and this soluble powder homogeneity is good.
Embodiment 2
A kind of florfenicol soluble powder, its preparation method is as follows:
1) join in the sodium hydroxide solution of 250gpH=8.5 by 20g florfenicol powder stock medicine and 5g Tween 80, stir 15min, mix homogeneously, obtains mixture A.
2) 1g dopamine hydrochloride is joined in mixture A, continue stirring 0.5 hour, obtain mixture B, mixture B is carried out spraying dry, controlling inlet temperature is 180 DEG C, leaving air temp 80 DEG C, peristaltic pump rotating speed 140rpm, obtains Powdered florfenicol and gathers dopamine complex, after testing, the drug loading that florfenicol gathers dopamine complex is 61.8%, and envelop rate is 88.5%.
3) content of the florfenicol gathered in the drug loading of dopamine complex and obtained florfenicol soluble powder according to florfenicol calculates the weight ratio that glucose and florfenicol gather dopamine complex.
4) weight ratio of gathering dopamine complex according to the glucose that calculates and florfenicol takes glucose and florfenicol gathers dopamine complex, again florfenicol is gathered dopamine complex and glucose is placed in mixer, stir 15min, mix homogeneously, namely obtained florfenicol weight percentage is the florfenicol soluble powder of 10% or 20%, and this soluble powder homogeneity is good.
Embodiment 3
A kind of florfenicol soluble powder, its preparation method is as follows:
1) join in the sodium hydroxide solution of 250gpH=8.5 by 20g florfenicol powder stock medicine, stir 15min, mix homogeneously, obtains mixture A.
2) 1g dopamine hydrochloride is joined in mixture A, continue stirring 2 hours, obtain mixture B, mixture B is carried out spraying dry, controlling inlet temperature is 160 DEG C, leaving air temp 90 DEG C, peristaltic pump rotating speed 140rpm, obtains Powdered florfenicol and gathers dopamine complex, after testing, the drug loading that florfenicol gathers dopamine complex is 55.7%, and envelop rate is 80.4%.
3) content of the florfenicol gathered in the drug loading of dopamine complex and obtained florfenicol soluble powder according to florfenicol calculates the weight ratio that glucose and florfenicol gather dopamine complex.
4) weight ratio of gathering dopamine complex according to the glucose that calculates and florfenicol takes glucose and florfenicol gathers dopamine complex, again florfenicol is gathered dopamine complex and glucose is placed in mixer, stir 15min, mix homogeneously, namely obtained florfenicol weight percentage is the florfenicol soluble powder of 10% or 20%, and soluble powder homogeneity is good.
In the present embodiment, glucose can replace with sucrose or maltodextrin, and the combination in any of maltodextrin, sucrose and glucose also can be used to replace.
Embodiment 4
A kind of florfenicol soluble powder, its preparation method is as follows:
1) join in the sodium hydroxide solution of 250gpH=8.5 by 20g florfenicol powder stock medicine and 5g PLURONICS F87, stir 15min, mix homogeneously, obtains mixture A.
2) 0.5g dopamine hydrochloride is joined in mixture A, continue stirring 1 hour, obtain mixture B, mixture B is carried out spraying dry, controlling inlet temperature is 170 DEG C, leaving air temp 85 DEG C, peristaltic pump rotating speed 140rpm, obtains Powdered florfenicol and gathers dopamine complex, after testing, the drug loading that florfenicol gathers dopamine complex is 52.7%, and envelop rate is 76.5%.
3) content of the florfenicol gathered in the drug loading of dopamine complex and obtained florfenicol soluble powder according to florfenicol calculates the weight ratio that maltodextrin and florfenicol gather dopamine complex.
4) weight ratio of gathering dopamine complex according to the maltodextrin that calculates and florfenicol takes maltodextrin and florfenicol gathers dopamine complex, again florfenicol is gathered dopamine complex and maltodextrin is placed in mixer, stir 15min, mix homogeneously, namely obtained florfenicol weight percentage is the florfenicol soluble powder of 10% or 20%, and soluble powder homogeneity is good.
In the present embodiment, maltodextrin can replace with sucrose or glucose, and the combination in any of maltodextrin, sucrose and glucose also can be used to replace.
Embodiment 5
A kind of florfenicol soluble powder, its preparation method is as follows:
1) join in the sodium hydroxide solution of 250gpH=8.5 by 20g florfenicol powder stock medicine and 2.5g PLURONICS F87, stir 15min, mix homogeneously, obtains mixture A.
2) 1g dopamine hydrochloride is joined in mixture A, continue stirring 2 hours, obtain mixture B, mixture B is carried out spraying dry, controlling inlet temperature is 170 DEG C, leaving air temp 85 DEG C, peristaltic pump rotating speed 140rpm, obtains Powdered florfenicol and gathers dopamine complex, after testing, the drug loading that florfenicol gathers dopamine complex is 58.5%, and envelop rate is 84.9%.
3) content of the florfenicol gathered in the drug loading of dopamine complex and obtained florfenicol soluble powder according to florfenicol calculates the weight ratio that sucrose and florfenicol gather dopamine complex.
4) weight ratio of gathering dopamine complex according to the sucrose that calculates and florfenicol takes sucrose and florfenicol gathers dopamine complex, again florfenicol is gathered dopamine complex and sucrose is placed in mixer, stir 15min, mix homogeneously, namely obtained florfenicol weight percentage is the florfenicol soluble powder of 10% or 20%, and soluble powder homogeneity is good.
In the present embodiment, sucrose can replace with maltodextrin or glucose, and the combination in any of maltodextrin, sucrose and glucose also can be used to replace.
Embodiment 6
A kind of florfenicol soluble powder, its preparation method is as follows:
1) join in the sodium hydroxide solution of 250gpH=8.5 by 20g florfenicol powder stock medicine and 5g PLURONICS F87, stir 15min, mix homogeneously, obtains mixture A.
2) 0.8g dopamine hydrochloride is joined in mixture A, continue stirring 0.5 hour, obtain mixture B, mixture B is carried out spraying dry, and controlling inlet temperature is 170 DEG C, leaving air temp 85 DEG C, peristaltic pump rotating speed 140rpm, obtain Powdered florfenicol and gather dopamine complex, the drug loading that florfenicol gathers dopamine complex is 53.3%, and envelop rate is 78.1%.
3) content of the florfenicol gathered in the drug loading of dopamine complex and obtained florfenicol soluble powder according to florfenicol calculates the weight ratio that glucose and florfenicol gather dopamine complex.
4) weight ratio of gathering dopamine complex according to the glucose that calculates and florfenicol takes glucose and florfenicol gathers dopamine complex, again florfenicol is gathered dopamine complex and glucose is placed in mixer, stir 15min, mix homogeneously, namely obtained florfenicol weight percentage is the florfenicol soluble powder of 10% or 20%, and soluble powder homogeneity is good.
In the present embodiment, glucose can replace with sucrose or maltodextrin, and the combination in any of maltodextrin, sucrose and glucose also can be used to replace.
Measure the dissolubility of florfenicol soluble powder of the present invention, for the florfenicol soluble powder that embodiment 1-6 is obtained, measurement result is as shown in table 1:
The dissolubility of the florfenicol soluble powder that table 1 embodiment 1-6 obtains compares
| 1000ppm | 2000ppm | 3000ppm | 4000ppm | |
| Embodiment 1 | Solution is clarified | Solution is clarified | Solution is clarified | Solution is slightly muddy |
| Embodiment 2 | Solution is clarified | Solution is clarified | Solution is slightly muddy | Solution is muddy |
| Embodiment 3 | Solution is clarified | Solution is slightly muddy | Solution is muddy | Solution is muddy |
| Embodiment 4 | Solution is clarified | Solution is slightly muddy | Solution is muddy | Solution is muddy |
| Embodiment 5 | Solution is clarified | Solution is clarified | Solution is slightly muddy | Solution is slightly muddy |
| Embodiment 6 | Solution is clarified | Solution is slightly muddy | Solution is slightly muddy | Solution is slightly muddy |
Concentration in table is with florfenicol gauge.
As shown in Table 1, the dissolubility of the florfenicol in the florfenicol soluble powder that embodiment 1 is obtained can up to 3000ppm.As can be seen here, the good water solubility of florfenicol soluble powder of the present invention, can be increased to 3000ppm by florfenicol solubility.
Florfenicol soluble powder soluble test
One, experiment material
1. main agents and medicine
Florfenicol soluble powder (being obtained by embodiment 1), 10% florfenicol powder (purchase of Zhejiang company)
2. major experimental equipment
Heat collecting type constant-temperature heating magnetic stirring apparatus Zhengzhou Greatwall Scientific Industrial & Trading Co., Ltd.
Two, test method
1. test group
Florfenicol weight percentage prepared by embodiment 1 is the novel florfenicol soluble powder of 10%.
2. matched group
From 10% florfenicol powder (be called for short like product, market is reflected the good product of water solublity) that Zhejiang company buys.
3. soluble test
Respectively 200mL distilled water is added in eight 250mL beakers, be placed in heat collecting type constant-temperature heating magnetic stirring apparatus heated constant temperature to 25 DEG C, the sample of test group added wherein in four beakers by following 4 concentration, the sample of matched group joins in another four beakers, observe dissolution phenomena, record reaches and dissolves terminal required time and phenomenon, the results are shown in Table 2.
Table 2 soluble test result
Above concentration is with florfenicol gauge.
As shown in Table 2, the present invention prepare florfenicol soluble powder dissolubility and dissolution rate apparently higher than other florfenicol soluble powders sold on the market, illustrate that florfenicol is gathered dopamine bag rear, its water solublity and dissolution rate are significantly improved, in actual applications, the dense demand of joining drinking water administration and using can be met.
The test of florfenicol soluble powder control animal large intestine bacillus mycoplasma infection
Certain pig farm natural occurrence, sick pig 194, is diagnosed as escherichia coli mycoplasma infection, and ill pig isolation is raised separately, ill swinery is equally divided into two groups and carries out treatment process:
Experimental group
Florfenicol percentage by weight prepared by embodiment 1 is the novel florfenicol soluble powder of 10%, mixed drink: in florfenicol, every 10g is watered 150kg, freely drinks, and is used in conjunction 3.
Drug control group
10% florfenicol powder (purchase of Zhejiang company), mixed drink: in florfenicol, every 10g is watered 150kg, freely drinks, and is used in conjunction 3.
Experimental result is as shown in table 3:
Table 3 florfenicol soluble powder is to swine escherichia coli mycoplasma infection therapeutic effect
As shown in Table 3, the cure rate that the florfenicol soluble powder that prepared by embodiment 1 controls swine escherichia coli mycoplasma infection than purchased florfenicol soluble powder is on the market high.As can be seen here, florfenicol soluble powder of the present invention is better than common commercial florfenicol soluble powder to the prevention effect of animal large intestine bacillus infection.
Claims (9)
1. a florfenicol soluble powder, is characterized in that gathering dopamine complex by florfenicol and matrix diluent forms:
The preparation method that described florfenicol gathers dopamine complex is as follows:
1) florfenicol powder is added in weak caustic solution, stirring and evenly mixing under room temperature, obtains mixture A; Or surfactant and florfenicol powder are added in weak caustic solution, stirring and evenly mixing under room temperature, obtain mixture A;
2) dopamine hydrochloride powder is joined in mixture A, wherein the mass ratio of florfenicol, dopamine hydrochloride, surfactant and weak caustic solution is 20:0.5-1:0-5:250, continue to stir 0.5-2 hour, obtain mixture B, mixture B is carried out spraying dry, obtains pulverous florfenicol and gather dopamine complex.
2. florfenicol soluble powder according to claim 1, is characterized in that: described weak caustic solution is the sodium hydroxide solution of pH=8.5.
3. florfenicol soluble powder according to claim 1, is characterized in that: described matrix diluent is any one in maltodextrin, dextrose plus saccharose, or 2-3 kind arbitrarily.
4. florfenicol soluble powder according to claim 3, is characterized in that: described matrix diluent is glucose.
5. florfenicol soluble powder according to claim 1, is characterized in that: described surfactant is PLURONICS F87 or Tween 80.
6. florfenicol soluble powder according to claim 1, is characterized in that: in described florfenicol soluble powder, the content of florfenicol is 10wt% or 20wt%.
7. florfenicol soluble powder according to claim 1, is characterized in that: step 2) in, spraying dry inlet temperature is 160 DEG C-180 DEG C, leaving air temp 80 DEG C-90 DEG C, peristaltic pump rotating speed 140rpm.
8. the preparation method of arbitrary described florfenicol soluble powder in claim 1-7, is characterized in that comprising the steps:
1) first measure florfenicol and gather the drug loading of dopamine complex, then calculated by the content of the florfenicol in this drug loading and required florfenicol soluble powder need to add matrix diluent, amount that florfenicol gathers dopamine complex;
2) florfenicol is gathered dopamine complex and matrix diluent is placed in mixer, stirring and evenly mixing, i.e. this florfenicol soluble powder obtained.
9. the preparation method of florfenicol soluble powder according to claim 8, is characterized in that: in obtained florfenicol soluble powder, the content of florfenicol is 10wt% or 20wt%.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106344516A (en) * | 2016-10-17 | 2017-01-25 | 安庆市柯旷动物药业有限公司 | Florfenicol powder |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0417572A2 (en) * | 1989-09-14 | 1991-03-20 | Massachusetts Institute Of Technology | Extended drug delivery of small, water-soluble molecules |
| CN101966340A (en) * | 2010-10-20 | 2011-02-09 | 无锡正大畜禽有限公司 | Method for producing florfenicol soluble powder |
| CN103920152A (en) * | 2014-04-25 | 2014-07-16 | 厦门大学 | Medicament based on multi-walled carbon nanotubes and preparation method of medicament |
-
2015
- 2015-12-25 CN CN201510996047.2A patent/CN105380909B/en active Active
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0417572A2 (en) * | 1989-09-14 | 1991-03-20 | Massachusetts Institute Of Technology | Extended drug delivery of small, water-soluble molecules |
| CN101966340A (en) * | 2010-10-20 | 2011-02-09 | 无锡正大畜禽有限公司 | Method for producing florfenicol soluble powder |
| CN103920152A (en) * | 2014-04-25 | 2014-07-16 | 厦门大学 | Medicament based on multi-walled carbon nanotubes and preparation method of medicament |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106344516A (en) * | 2016-10-17 | 2017-01-25 | 安庆市柯旷动物药业有限公司 | Florfenicol powder |
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Inventor after: Zhang Weiyuan Inventor after: Huang Wenhui Inventor after: Li Zibin Inventor after: Tang Wanyong Inventor after: Ding Wenge Inventor after: Zhang Cuiping Inventor after: Zhang Yongdan Inventor after: Liu Zhibin Inventor after: Zhu Xiugao Inventor after: Yu Hujie Inventor before: Zhang Weiyuan Inventor before: Huang Wenhui Inventor before: Li Zibin Inventor before: Tang Wanyong Inventor before: Ding Wenge Inventor before: Zhang Cuiping Inventor before: Zhang Yongdan Inventor before: Liu Zhibin Inventor before: Zhu Xiugao Inventor before: Yu Hujie |
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